Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons

Blackwell, Raymond E.; Zhao, Fangzhou; Brooks, Erin; Zhu, Junmian; Piskun, Ilya; Wang, Shenkai; Delgado, Aidan; Lee, Yea-Lee; Louie, Steven G.; Fischer, Felix R.

doi:10.1038/s41586-021-04201-y

Title: Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons

Journal Article · Wed Dec 22 00:00:00 EST 2021 · Nature (London)

DOI:https://doi.org/10.1038/s41586-021-04201-y· OSTI ID:1900420

Blackwell, Raymond E. ^[1]; Zhao, Fangzhou ^[2];

^[1]; Zhu, Junmian ^[1]; Piskun, Ilya ^[1]; Wang, Shenkai ^[1]; Delgado, Aidan ^[1]; Lee, Yea-Lee ^[1];

^[2];

^[3]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)

Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena that have sparked renewed interest in carbon-based spintronics. Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases and even metallic zero mode bands, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Finally, our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF); Center for Energy Efficient Electronics Science; National Institutes of Health (NIH)

Grant/Contract Number:: AC02-05CH11231; N00014-19-1-2503; DMR-1839098; DMR-1926004; ECCS-0939514; N00014-16-1-2921; DGE-11064000; S10OD024998

OSTI ID:: 1900420

Journal Information:: Nature (London), Vol. 600, Issue 7890; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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